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基于原位接枝季銨鹽抗菌材料的制備及其抗菌性能研究

發(fā)布時(shí)間:2018-05-04 08:57

  本文選題:碳納米管 + 聚丙烯纖維 ; 參考:《西南交通大學(xué)》2017年碩士論文


【摘要】:材料表面極易生長各種有害細(xì)菌,不僅容易引起材料污損和生物腐蝕等,其快速和大量繁殖還會對人類的健康和生存環(huán)境造成威脅。因此材料表面的抗菌功能修飾逐漸受到越來越廣泛的重視。常見的材料抗菌改性技術(shù)主要包括表面涂覆抗菌涂層,復(fù)合添加抗菌劑以及通過材料表面化學(xué)接枝抗菌成分等。雖然表面涂覆和物理共混的制備方法簡單,但抗菌劑的釋放量會逐漸降低并存在微生物耐抗藥性等問題;相比而言,表面化學(xué)接枝抗菌劑是獲得長效穩(wěn)定抗菌性能的有效方法。相對于有機(jī)小分子和無機(jī)抗菌劑,高分子抗菌劑具有更多的活性官能團(tuán),且化學(xué)穩(wěn)定性好,可避免殘余毒性。因此將高分子抗菌劑通過簡單的方法化學(xué)接枝到材料表面具有重要意義。本論文主要針對材料表面涂覆和物理添加抗菌成分后抗菌性能不穩(wěn)定和長效差等問題,以碳納米管(CNTs)和聚丙烯(PP)纖維作為改性對象,通過原位季銨化和紫外光引發(fā)原位自由基聚合兩種方法接枝高分子季銨鹽,獲得抗菌材料的探索性研究。探討了季銨化前驅(qū)體添加量及分子量、聚合反應(yīng)單體和引發(fā)劑的添加量等因素對季銨鹽接枝效果和對材料結(jié)構(gòu)的影響,并研究了改性材料的抗菌性能。1.通過在酸化CNTs表面接枝聚乙烯亞胺(PEI),再對PEI進(jìn)行季銨化制備表面接枝高分子季銨鹽的碳納米管(QPEI@CNTs),并通過溶劑蒸發(fā)法制備了QPEI@CNTs/PLA復(fù)合膜以考察其分散性。結(jié)果表明,季銨基團(tuán)的引入顯著增加了 CNTs對革蘭氏陰性菌和革蘭氏陽性菌菌株的抗菌活性,并提高了 CNTs在聚乳酸(PLA)中的分散性。當(dāng)PEI分子量為70000,與碳納米管的配比為3:1時(shí),其對代表性實(shí)驗(yàn)菌株的最小抑菌濃度(MIC)可以分別達(dá)到20-50mg/L(大腸桿菌,Ecoli)和50-100mg/L(金黃色葡萄球菌,Saureus)。2.設(shè)計(jì)小分子季銨鹽甲基丙烯酰氧乙基-芐基-二甲基氯化銨(MBDAC)在光活性劑二苯甲酮經(jīng)紫外光激發(fā)下,在PP纖維表面發(fā)生原位自由基聚合反應(yīng),獲得表面接枝高分子季銨鹽的改性PP纖維(PMBDAC@PP)。表征結(jié)果表明,PMBDAC@PP纖維表面生成了大量活性官能團(tuán),使PP纖維表面由疏水性變?yōu)橛H水性,季銨鹽基團(tuán)賦予PP纖維良好的抗菌性能;12.68%接枝量的PP纖維對Ecoli和S.aureus的抗菌率均達(dá)到了99%以上。3.以丙烯酸為單體,通過紫外光引發(fā)自由基原位聚合反應(yīng)在PP纖維表面接枝聚丙烯酸,隨后通過酰胺化反應(yīng)接枝殼聚糖,并通過(2,3環(huán)氧丙基)三甲基氯化銨(ETA)開環(huán)反應(yīng)對其季銨化,制備得到表面接枝殼聚糖季銨鹽的PP纖維(QCH@PP-AA)。研究發(fā)現(xiàn),QCH@PP-AA纖維相對于表面僅接枝殼聚糖的CH@PP-AA纖維,對E.coli和S.aureus具有更優(yōu)異的抗菌性能,3.51%接枝改性的PP纖維,其對兩種代表性試驗(yàn)菌株的抗菌率可以達(dá)到98%以上。
[Abstract]:All kinds of harmful bacteria are easily grown on the surface of the material, which can not only cause material fouling and biological corrosion, but also threaten the health and living environment of human being. Therefore, the antibacterial function modification of the material surface has gradually been paid more and more attention. The common materials for antibacterial modification include surface coating. In addition to the simple preparation method of surface coating and physical blending, the release amount of the antibacterial agent will gradually decrease and the antimicrobial resistance of the microorganisms exist. In comparison, the surfactants graft antibacterial agent is a long-term and stable antibacterial property. Effective methods. Relative to organic small molecules and inorganic antibacterial agents, polymer antibacterial agents have more active functional groups, and have good chemical stability and can avoid residual toxicity. Therefore, it is of great significance to graft polymer antibacterial agents into the surface of materials by simple methods. The antibacterial properties are unstable and the long effect is poor. Using the carbon nanotube (CNTs) and the polypropylene (PP) fiber as the modified objects, two kinds of quaternary ammonium salts are grafted by in situ quaternizing and UV irradiation in situ free radical polymerization. The exploration of the antibacterial materials is obtained. The amount and the molecular weight of the quaternized precursor are discussed. The effect of the grafting effect of quaternary ammonium salt and the effect on the structure of the material of the quaternary ammonium salt, such as the quantity, the polymerization of the monomer and the initiator, and the study of the antibacterial properties of the modified material.1. by grafting polyethyleneimine (PEI) on the surface of the acidified CNTs, and the preparation of the carbon nanotubes (QPEI@CNTs) to prepare the surface graft polymer quaternary ammonium salt by quaternizing of PEI and through the preparation of the modified carbon nanotubes (QPEI@CNTs). QPEI@CNTs/PLA composite membrane was prepared by solvent evaporation to investigate its dispersibility. The results showed that the introduction of quaternary ammonium group significantly increased the antibacterial activity of CNTs to gram-negative and Gram-positive bacteria, and increased the dispersion of CNTs in polylactic acid (PLA). When the molecular weight of PEI was 70000 and the ratio of carbon nanotubes was 3:1, The minimum inhibitory concentration (MIC) of the representative experimental strains (MIC) can be reached to 20-50mg/L (Escherichia coli, Ecoli) and 50-100mg/L (Staphylococcus aureus, Saureus).2. design small molecule quaternary ammonium salt methyl acryroethoxy benzyl two methyl ammonium chloride (MBDAC) on the surface of PP fiber on the surface of PP fiber under the UV excitation of the PHOTOACTIVATOR two benzophenone. In situ free radical polymerization, the modified PP fiber (PMBDAC@PP) on the surface graft polymer quaternary ammonium salt was obtained. The results showed that a large number of active functional groups were formed on the surface of PMBDAC@PP fibers, which made the surface of PP fibers from hydrophobicity to hydrophilic, and the quaternary ammonium group gave PP fiber good antibacterial properties, and the PP fiber of 12.68% grafting amount to Ecoli and S.. The antibacterial rate of aureus reached more than 99%.3. with acrylic acid as a monomer. The graft copolymerization of polyacrylic acid on the surface of PP fiber by UV irradiation was carried out on the surface of PP fiber. Then the chitosan was grafted by amidation, and the surface graft copolymerization was prepared by the (2,3 epoxy propyl) three methyl ammonium chloride (ETA) ring opening reaction. PP fiber (QCH@PP-AA) of sugar quaternary ammonium salt. It is found that the QCH@PP-AA fiber has better antibacterial properties to E.coli and S.aureus than the CH@PP-AA fiber that is only grafted with chitosan on the surface. The antibacterial rate of the 3.51% graft modified PP fibers can reach more than 98% for the two representative test strains.

【學(xué)位授予單位】:西南交通大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:TB34

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